Extended star graph as a light-harvesting-complex prototype: Excitonic absorption speedup by peripheral energy defect tuning.

Abstract

We study the quantum dynamics of a photoexcitation uniformly distributed at the periphery of an extended star network (with N_{B} branches of length L_{B}). More specifically, we address here the question of the energy absorption at the core of the network and how this process can be improved (or not) by the inclusion of peripheral defects with a tunable energy amplitude Δ. Our numerical simulations reveal the existence of optimal value of energy defect Δ^{*} which depends on the network architecture. Around this value, the absorption process presents a strong speedup (i.e., reduction of the absorption time) provided that L_{B}≤L_{B}^{*} with L_{B}^{*}≈12.5/ln(N_{B}). Analytical and numerical developments are then conducted to interpret this feature. We show that the origin of this speedup takes place in the hybridization of two upper-band excitonic eigenstates. This hybridization is important when L_{B}≤L_{B}^{*} and vanishes almost totally when L_{B}>L_{B}^{*}. These structural rules we draw here could represent a potential guide for the practical design of molecular nanonetwork dedicated to the realization of efficient photoexcitation absorption.